Novel silver/silver molybdate（Ag/Ag2MoO4） composites with surface plasmon resonance（SPR）-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence o...Novel silver/silver molybdate（Ag/Ag2MoO4） composites with surface plasmon resonance（SPR）-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence of sodium dodecyl sulfate（SDS） in this study.The as prepared silver/silver molybdate（Ag/Ag2MoO4） composites were systematically characterized by X-ray diffraction（XRD）,scanning electron microscopy（SEM） and ultraviolet-visible diffuse reflectance absorption spectroscopy（DRS） in order to investigate their crystal structure,morphology and optical property as well.The photocatalytic activities of the composites were subsequently evaluated by their ability to degrade rhodamine B（RhB） under visible-light irradiation.Varies of controlled experiments were then carefully operated to gain a deep insight into the assembling of Ag/Ag2MoO4composites.It was found that preparation conditions such as pH,reaction time,and the amount of surfactant played important roles in the formation of composites with octahedral microstructures.And the composite obtained at 160 ℃ using 0.5 g of sodium dodecyl sulfate exhibited the highest photocatalytic performance under visible-light irradiation.Capture experiments were also conducted to clarify the function of different active species generated on the surface of Ag/Ag2MoO4during the photocatalytic process,in which both holes and ·OH radicals were found to play crucial role in photocatalytic removal of RhB under visible light irradiation.A possible photocatalytic mechanism of Ag/Ag2MoO4 was finally proposed on the basis of all the results to explain the higher photocatalytic activity of the octahedral Ag/Ag2MoO4 composites.It was inferred that the photoinduced ＂hot＂ electrons can quickly transfer from the Ag NPs to the conduction band of Ag2MoO4 and react with oxygen and H2O to generate a large quality of active radicals such as ·OH and ·O2^- because of the SPR effects.Besides,this SPR effects of Ag nanoparticles deposited on the surface of Ag2MoO4 can not only dramatically amplify its light absorption,especially in the visible region,but also promote the separation of photoexcited electron-hole pairs and effectively decrease electron-hole recombination.展开更多
Silver nanoplates,with average thickness about 5 nm and average tunable size from 40 to 500 nm,were synthesized via a simple room-temperature solution-phase chemical reduction method in the presence of appropriate con...Silver nanoplates,with average thickness about 5 nm and average tunable size from 40 to 500 nm,were synthesized via a simple room-temperature solution-phase chemical reduction method in the presence of appropriate concentration of trisodium citrate and silver seeds.The optical in-plane dipole plasmon resonance bands of these silver plates could be tuned from 520 to 1100 nm.Control experiments were explored for understanding of the growth mechanism.It is found that both the amount of citrate ions and the small silver seeds added to the growth solution are the key to controlling the silver nanoplates without changing their thickness and crystal structure.Small silver seeds are found to play an important role in the formation of large thin silver nanoplates when poly（vinylpyrrolidone）（PVP） are used as capping agent.展开更多
Triangular Au-Ag framework nanostructures （TFN） were synthesized via a multi-step galvanic replacement reaction （MGRR） of single-crystalline triangular silver nanoplates in a chlorauric acid （HAuCl4） solution at...Triangular Au-Ag framework nanostructures （TFN） were synthesized via a multi-step galvanic replacement reaction （MGRR） of single-crystalline triangular silver nanoplates in a chlorauric acid （HAuCl4） solution at room temperature. The morphological, compositional, and crystal structural changes involved with reaction steps were analyzed by using transmission electron microscopy（TEM）, energy-dispersive X-ray spectrometry （EDX）, and X-ray diffraction. TEM combined with EDX and selected area electron diffraction confirmed the replacement of Ag with Au. The in-plane dipolar surface plasmon resonance （SPR） absorption band of the Ag nanoplates locating initially at around 700 nm gradually redshifted to 1 100 nm via a multi-stage replacement manner after 7 stages. The adding amount of HAuCl4 per stage influenced the average redshift value per stage, thus enabled a fine tuning of the in-plane dipolar band. A proposed formation mechanism of the original Ag nanoplates developing pores while growing Au nanoparticles covering this underlying structure at more reaction steps was confirmed by exploiting surface-enhanced Raman scattering （SERS）.展开更多
Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the ox...Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide（NO） under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.展开更多
Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, o...Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, oxygen vacancies, Bi particles, and Bi2O2CO3 were co-induced in BiOI via a facile in situ assembly method at room temperature using NaBH4 as the reducing agent. In the synthesized ternary Bi/BiOI/(BiO)2CO3, the oxygen vacancies, dual heterojunctions (i.e., Bi/BiOI and Bi- OI/(BiO)2CO3), and surface plasmon resonance effect of the Bi particles contributed to efficient electron-hole separation and an increase in charge carrier concentration, thus boosting the overall visible light photocatalysis efficiency. The as-prepared catalysts were applied for the removal of NO in concentrations of parts per billion from air in continuous air flow under visible light illumination. Bi/BiOI/(BiO)2CO3 exhibited a highly enhanced NO removal ratio of 50.7%, much higher than that of the pristine BiOI (1.2%). Density functional theory calculations and experimental results revealed that the Bi/BiOI/(BiO)2CO3 composites promoted the production of reactive oxygen species for photocatalytic NO oxidation. Thus, this work provides a new strategy to modify narrow-band semiconductors and explore other bismuth-containing heterostructured visible-light-driven photocatalysts.展开更多
Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advanta...Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.展开更多
Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode ...Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.展开更多
The photocatalytic reduction of CO2 with H2O to fuels and chemicals using solar energy is one of the most attractive but highly difficult routes.Thus far,only a very limited number of photocatalysts has been reported ...The photocatalytic reduction of CO2 with H2O to fuels and chemicals using solar energy is one of the most attractive but highly difficult routes.Thus far,only a very limited number of photocatalysts has been reported to be capable of catalyzing the photocatalytic reduction of CO2 under visible light.The utilization of the localized surface plasmon resonance(LSPR)phenomenon is an attractive strategy for developing visible-light photocatalysts.Herein,we have succeeded in synthesizing plasmonic MoO3?x-TiO2 nanocomposites with tunable LSPR by a simple solvothermal method.The well-structured nanocomposite containing two-dimensional(2D)molybdenum oxide(MoO3?x)nanosheets and one-dimensional(1D)titanium oxide nanotubes(TiO2-NT)showed LSPR absorption band in the visible-light region,and the incorporation of TiO2-NT significantly enhanced the LSPR absorption band.The MoO3?x-TiO2-NT nanocomposite is promising for application in the photocatalytic reduction of CO2 with H2O under visible light irradiation.展开更多
Sliver nanoplates were prepared through a visible light induced reduction process by a reaction between sodium citrate and silver nitrate in an aqueous solvent at room temperature. UV-Vis spectra were employed to moni...Sliver nanoplates were prepared through a visible light induced reduction process by a reaction between sodium citrate and silver nitrate in an aqueous solvent at room temperature. UV-Vis spectra were employed to monitor the growth of the silver nanoplates. The resulting spectra indicated that, at an early stage, the products were spherical particles with planar nanoparticles appearing and growing subsequently. In the last stages of the process, some spherical particles were consumed by the growth of the nanoparticles, through an Ostwald ripening mechanism. Furthermore, it was found that the addition of either Poly（Vinyl Pyrrolidone） （PVP） or excessive citrate could stabilize the colloidal system effectively, and that rigorous stirring was necessary for the anticipant products, Introduction of a large quantities of sodium hydroxide can dramatically accelerate the reactive rate of the photoreduction process.展开更多
Triangular silver nanoplates in aqueous solvent and on the surface of quartz substrate have been synthesized by seed-mediated growth approach in the presence of tannin.It was found that both the amount of tannin and t...Triangular silver nanoplates in aqueous solvent and on the surface of quartz substrate have been synthesized by seed-mediated growth approach in the presence of tannin.It was found that both the amount of tannin and the small triangular silver nanoplate seeds added to the growth solution are the key factors to modulation absorption band of triangular silver nanoplates.The optical in-plane dipole surface plasmon resonance (SPR) bands of these Ag nanoplates can be tuned from 608 nm to 980 nm via tannin deoxidization method.The formation mechanism of triangular silver nanoplates was proposed.The tannin deoxidization method realizes a convenient modulation of the absorption band of Ag nanostructures within the visible near-infrared (IR) region both in aqueous solvent and on substrates under mild conditions.展开更多
Despite of extensive attention on the copper-based heterogeneous oxidative homocoupling of alkynes(OHA)to 1,3-diynes,the photocatalytic OHA is scarcely investigated.By screening copper-containing spinel catalysts,we d...Despite of extensive attention on the copper-based heterogeneous oxidative homocoupling of alkynes(OHA)to 1,3-diynes,the photocatalytic OHA is scarcely investigated.By screening copper-containing spinel catalysts,we discovered that a prereduced copper ferrite(CuFe2O4)not only can catalyze the thermocatalytic OHA but also is efficient for the photocatalytic OHA under visible light irradiation.It is found that the sol-gel combustion(SG)method and the partial reduction at 250 ℃ can result in the optimal CuFe2O4-SG-250 catalyst showing high activity and stability.Surface oxidized Cu2O is evidenced to be the active species for the thermocatalytic OHA,whereas metallic copper nanopaticles(CuNPs)are identified as the active sites for the photocatalytic OHA.The efficiency of photocatalytic OHA at ambient temperature is comparable to that of thermocatalytic OHA at 120 ℃,and the CuFe2O4-SG-250 catalyst can be magnetically separated and reused at least five times.The localized surface plasmon resonance effect of CuNPs contributes to visible light-induced photocatalytic OHA.展开更多
Non-stoichiometric W_(18)O_(49)(WO)prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies.This has great potential in the field of...Non-stoichiometric W_(18)O_(49)(WO)prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies.This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels.In addition,through the amination of CdSe,the one-dimensional/two-dimensional step-scheme(S-scheme)WO/CdSe-diethylenetriamine(WO/CdSe-D)photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method.The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency.The optimized photocatalyst of 35%WO/CdSe-D has the best CO_(2) reduction performance compared to WO and CdSe-D,and the yield is 25.37μmol h^(–1) g^(–1).X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction.This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO_(2) reduction.展开更多
Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,f...Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol(BA)into benzaldehydes(BAD)and H_(2),a novel localized surface plasmon resonance(LSPR)enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_(3-x) as oxidation semiconductor and Zn_(0.1)Cd_(0.9)S as reduction semiconductor.The photoredox system of Zn_(0.1)Cd_(0.9)S/MoO_(3-x) displayed an unconventional reaction model,in which the BA served as both electron donor and acceptor.The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically.Moreover,due to the LSPR effect of MoO_(3-x) nanosheets,Zn_(0.1)Cd_(0.9)S/MoO_(3-x) photocatalysts exhibited strong absorption in the region of full solar spectrum.Therefore,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite generated H_(2) and BAD simultaneously via selective oxidation of BA with high production(34.38 and 33.83 mmol×g^(–1) for H_(2) and BAD,respectively)upon full solar illumination.Even under NIR light irradiation,the H_(2) production rate could up to 94.5 mmol×g^(–1)×h^(–1).In addition,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite displayed effective photocatalytic H_(2) evolution rate up to 149.2 mmol×g^(–1)×h^(–1) from water,which was approximate 6 times that of pure Zn_(0.1)Cd_(0.9)S.This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.展开更多
A fast and facile method of fabricating fiber-optic localized surface plasmon resonance sensors baseff on spherical gold nanoparticles was introduced in this study. The gold nanoparticles with an average diameter of 5...A fast and facile method of fabricating fiber-optic localized surface plasmon resonance sensors baseff on spherical gold nanoparticles was introduced in this study. The gold nanoparticles with an average diameter of 55 nm were synthesized via the Turkevich method and were then immobilized onto the surface of an uncladded sensor probe using a polydopamine layer. To obtain a sensor probe with high sensitivity to changes in the refractive index, a set of key optimization parameters, including the sensing length, coating time of the potydopamine layer, and coating time of the gold nanoparticles, were investigated. The sensitivity of the optimized sensor probe was 522.80 nm per refractive index unit, and the probe showed distinctive wavelength shifts when the refractive index was changed from 1.328 6 to 1.398 7. When stored in deionized water at 4 ℃, the sensor probe proved to be stable over a period of two weeks. The sensor also exhibited advantages, such as low cost, fast fabrication, and simple optical setup, which indicated its potential application in remote sensing and real-time detection.展开更多
Lipoic acid (LA) has received great attention in the area of gold surface functionalization. In this study, LA was employed as a linker for the attachment of antibody to the gold surface of surface plasmon resonance (...Lipoic acid (LA) has received great attention in the area of gold surface functionalization. In this study, LA was employed as a linker for the attachment of antibody to the gold surface of surface plasmon resonance (SPR) chip. By using this chip in a homemade SPR immunosensor, low molecular weight compound 2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD) can be detected at a low level of 0.01 ng/mL. There is a good linear relationship(R2 =0.943 1) between the results of SPR biosensor and enzyme-linked immunosorbent assay(ELISA).展开更多
To perform the mechanism study of special association for vancomycin and D-Ala-D-Ala-containing peptides on the interface of solution and self-assemble monolayer, the binding between vancomycin and pentapeptide （Lys-...To perform the mechanism study of special association for vancomycin and D-Ala-D-Ala-containing peptides on the interface of solution and self-assemble monolayer, the binding between vancomycin and pentapeptide （Lys-Lys-Gly-D-Ala-D-Ala） was investigated by flow injection surface plasmon resonance （FI-SPR） and flow injection quartz crystal microbalance （FI-QCM）. To facilitate the formation of a compact vancomycin adsorbates layer with a uniform surface orientation, vancomycin molecules were attached onto a preformed alkanethiol self-assembled monolayer. By optimizing the conditions for the binding between Lys-Lys-Gly-D-Ala-D-Ala and vancomycin on the assembled chip, the detecting limit of Lys-Lys-Gly-D-Ala-D-Ala was greatly improved （reaching 0.5 ×10^- 6 mol/L or 7.5 × 10^-12 mol）. The equilibrium constant of the association of Lys-Lys-Gly-D-Ala-D-Ala with vancomycin was also obtained （KAds=5.0×10^4 L/tool）.展开更多
The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon ...The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon resonance of small metallic particles. The role of energy transfer between ions and the particle is theoretical discussed. Depending on the particle size and the ion emission quantum efficiency, the enhancement of the absorption and the fluorescence is predicted. Moreover, taking Yb^3＋-doped ZBLAN as example, the cooling power and heat-light converting efficiency are calculated. It is finally concluded that the absorption and the fluorescence are greatly enhanced in these composite materials, the cooling power is increased compared to the bulk material.展开更多
The n-type semiconducting titanium oxide thin films are well-known as electron transporting interlayer in photovoltaic cells. The favorable characteristics of interlayers in photovoltaics are high optical transmittan...The n-type semiconducting titanium oxide thin films are well-known as electron transporting interlayer in photovoltaic cells. The favorable characteristics of interlayers in photovoltaics are high optical transmittance （T%）, wide band gap energy （Eg） and high electrical conductivity （σ）. Modifying titanium oxide films with metal nanoparticles would increase electrical conductivity but reduce optical band gap energy. We developed the sol-gel derived titanium suboxide （TiOx） films modified with silver （Ag） or gold （Au） or copper （Cu） nanoparticles （NPs）. This study explores a tradeoff between narrowing optical band gap and enhancing electrical conductivity of nanostructured TiOx films by controlling the Au- or Ag- or Cu-NPs loading concentrations （mol%） in titania. The Au- and Cu-NPs loading concentration of 4 mol% should meet a tradeoff which yields the higher T%, wider Eg and higher compared to those of pure TiOx films. In addition, since the pure Cu is not thermodynamically stable in ambience as compared to Au and Ag, the stability of as-obtained colloidal CuNPs is also examined. A careful examination of the time evolution of surface plasmon resonance （SPR） bands of CuNPs indicates that their stability is only up to 4 h.展开更多
Baicalein, baicalin, scutellarin and Chrysin-7-O-β-D-glucuronide are the major flavonoids of the Shuang-huang-lian powder injection. These flavonoids are thought to be haptens that can induce allergic reactions. The ...Baicalein, baicalin, scutellarin and Chrysin-7-O-β-D-glucuronide are the major flavonoids of the Shuang-huang-lian powder injection. These flavonoids are thought to be haptens that can induce allergic reactions. The interaction mechanism of these haptens with bovine serum albumin （BSA） was investigated by surface plasmon resonance （SPR） and molecular modeling method. The SPR study indicated that these compounds could specifically bind to the BSA with one binding site and equilibrium dissociation constant （KD） values were determined. Molecular modeling explored the mechanism of interaction under simulated physiological condition. The result of molecular modeling indicated that flavonoids could bind with BSA in the hydrophobic pocket of sub-domain II with hydrogen bonding as the main acting force.展开更多
基金supported by Fundamental Research Funds for the Central Universities (2662014BQ061, 2015PY120, 2015PY047, 2016PY088)the National Natural Science Foundation of China (51572101, 21502059, 21607047)~~
文摘Novel silver/silver molybdate（Ag/Ag2MoO4） composites with surface plasmon resonance（SPR）-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence of sodium dodecyl sulfate（SDS） in this study.The as prepared silver/silver molybdate（Ag/Ag2MoO4） composites were systematically characterized by X-ray diffraction（XRD）,scanning electron microscopy（SEM） and ultraviolet-visible diffuse reflectance absorption spectroscopy（DRS） in order to investigate their crystal structure,morphology and optical property as well.The photocatalytic activities of the composites were subsequently evaluated by their ability to degrade rhodamine B（RhB） under visible-light irradiation.Varies of controlled experiments were then carefully operated to gain a deep insight into the assembling of Ag/Ag2MoO4composites.It was found that preparation conditions such as pH,reaction time,and the amount of surfactant played important roles in the formation of composites with octahedral microstructures.And the composite obtained at 160 ℃ using 0.5 g of sodium dodecyl sulfate exhibited the highest photocatalytic performance under visible-light irradiation.Capture experiments were also conducted to clarify the function of different active species generated on the surface of Ag/Ag2MoO4during the photocatalytic process,in which both holes and ·OH radicals were found to play crucial role in photocatalytic removal of RhB under visible light irradiation.A possible photocatalytic mechanism of Ag/Ag2MoO4 was finally proposed on the basis of all the results to explain the higher photocatalytic activity of the octahedral Ag/Ag2MoO4 composites.It was inferred that the photoinduced ＂hot＂ electrons can quickly transfer from the Ag NPs to the conduction band of Ag2MoO4 and react with oxygen and H2O to generate a large quality of active radicals such as ·OH and ·O2^- because of the SPR effects.Besides,this SPR effects of Ag nanoparticles deposited on the surface of Ag2MoO4 can not only dramatically amplify its light absorption,especially in the visible region,but also promote the separation of photoexcited electron-hole pairs and effectively decrease electron-hole recombination.
基金Project (10804101) supported by the National Nature Science Foundation of ChinaProject (2007CB815102) supported by the National Basic Research Program of ChinaProject (2007B08007) supported by the Science and Technology Development Foundation of Chinese Academy of Engineering Physics
文摘Silver nanoplates,with average thickness about 5 nm and average tunable size from 40 to 500 nm,were synthesized via a simple room-temperature solution-phase chemical reduction method in the presence of appropriate concentration of trisodium citrate and silver seeds.The optical in-plane dipole plasmon resonance bands of these silver plates could be tuned from 520 to 1100 nm.Control experiments were explored for understanding of the growth mechanism.It is found that both the amount of citrate ions and the small silver seeds added to the growth solution are the key to controlling the silver nanoplates without changing their thickness and crystal structure.Small silver seeds are found to play an important role in the formation of large thin silver nanoplates when poly（vinylpyrrolidone）（PVP） are used as capping agent.
基金Project(10804101)supported by the National Natural Science Foundation of ChinaProject(2007CB815102)supported by the National Basic Research Program of ChinaProject(2007B08007)supported by the Science and Technology Development Foundation of Chinese Academy of Engineering Physics,China
文摘Triangular Au-Ag framework nanostructures （TFN） were synthesized via a multi-step galvanic replacement reaction （MGRR） of single-crystalline triangular silver nanoplates in a chlorauric acid （HAuCl4） solution at room temperature. The morphological, compositional, and crystal structural changes involved with reaction steps were analyzed by using transmission electron microscopy（TEM）, energy-dispersive X-ray spectrometry （EDX）, and X-ray diffraction. TEM combined with EDX and selected area electron diffraction confirmed the replacement of Ag with Au. The in-plane dipolar surface plasmon resonance （SPR） absorption band of the Ag nanoplates locating initially at around 700 nm gradually redshifted to 1 100 nm via a multi-stage replacement manner after 7 stages. The adding amount of HAuCl4 per stage influenced the average redshift value per stage, thus enabled a fine tuning of the in-plane dipolar band. A proposed formation mechanism of the original Ag nanoplates developing pores while growing Au nanoparticles covering this underlying structure at more reaction steps was confirmed by exploiting surface-enhanced Raman scattering （SERS）.
基金supported by the National Program on Key Basic Research Project (2016YFA0203000)the Early Career Scheme (ECS 809813) from the Research Grant Council, Hong Kong SAR Government+2 种基金the Croucher Foundation Visitorship for PRC Scholars 2015/16 at The Education University of Hong Kongthe National Natural Science Foundation of China (51672312, 21373275)the Program for New Century Excellent Talents in University (NCET-12-0668)~~
文摘Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide（NO） under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.
基金supported by the National Natural Science Foundation of China(21501016,21777011,51871037,51501024)the Innovative Research Team of Chongqing(CXTDG201602014)+1 种基金the Key Natural Science Foundation of Chongqing(cstc2017jcyjBX0052)the Plan for "National Youth Talents" of the Organization Department of the Central Committee~~
文摘Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, oxygen vacancies, Bi particles, and Bi2O2CO3 were co-induced in BiOI via a facile in situ assembly method at room temperature using NaBH4 as the reducing agent. In the synthesized ternary Bi/BiOI/(BiO)2CO3, the oxygen vacancies, dual heterojunctions (i.e., Bi/BiOI and Bi- OI/(BiO)2CO3), and surface plasmon resonance effect of the Bi particles contributed to efficient electron-hole separation and an increase in charge carrier concentration, thus boosting the overall visible light photocatalysis efficiency. The as-prepared catalysts were applied for the removal of NO in concentrations of parts per billion from air in continuous air flow under visible light illumination. Bi/BiOI/(BiO)2CO3 exhibited a highly enhanced NO removal ratio of 50.7%, much higher than that of the pristine BiOI (1.2%). Density functional theory calculations and experimental results revealed that the Bi/BiOI/(BiO)2CO3 composites promoted the production of reactive oxygen species for photocatalytic NO oxidation. Thus, this work provides a new strategy to modify narrow-band semiconductors and explore other bismuth-containing heterostructured visible-light-driven photocatalysts.
基金supported by the National Natural Science Foundation of China(21501016,21777011 and 21822601)the National Key R&D Program of China(2016YFC02047)+2 种基金the Innovative Research Team of Chongqing(CXTDG201602014)the Key Natural Science Foundation of Chongqing(cstc2017jcyj BX0052)the National Ten Thousand Talent Program of China~~
文摘Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.
文摘Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.
文摘The photocatalytic reduction of CO2 with H2O to fuels and chemicals using solar energy is one of the most attractive but highly difficult routes.Thus far,only a very limited number of photocatalysts has been reported to be capable of catalyzing the photocatalytic reduction of CO2 under visible light.The utilization of the localized surface plasmon resonance(LSPR)phenomenon is an attractive strategy for developing visible-light photocatalysts.Herein,we have succeeded in synthesizing plasmonic MoO3?x-TiO2 nanocomposites with tunable LSPR by a simple solvothermal method.The well-structured nanocomposite containing two-dimensional(2D)molybdenum oxide(MoO3?x)nanosheets and one-dimensional(1D)titanium oxide nanotubes(TiO2-NT)showed LSPR absorption band in the visible-light region,and the incorporation of TiO2-NT significantly enhanced the LSPR absorption band.The MoO3?x-TiO2-NT nanocomposite is promising for application in the photocatalytic reduction of CO2 with H2O under visible light irradiation.
文摘Sliver nanoplates were prepared through a visible light induced reduction process by a reaction between sodium citrate and silver nitrate in an aqueous solvent at room temperature. UV-Vis spectra were employed to monitor the growth of the silver nanoplates. The resulting spectra indicated that, at an early stage, the products were spherical particles with planar nanoparticles appearing and growing subsequently. In the last stages of the process, some spherical particles were consumed by the growth of the nanoparticles, through an Ostwald ripening mechanism. Furthermore, it was found that the addition of either Poly（Vinyl Pyrrolidone） （PVP） or excessive citrate could stabilize the colloidal system effectively, and that rigorous stirring was necessary for the anticipant products, Introduction of a large quantities of sodium hydroxide can dramatically accelerate the reactive rate of the photoreduction process.
基金Project(10804101) supported by the National Natural Science Foundation of ChinaProject(2007CB815102) supported by the National Basic Research Program of ChinaProject(2007B08007) supported by the Science and Technology Development Foundation of Chinese Academy of Engineering Physics
文摘Triangular silver nanoplates in aqueous solvent and on the surface of quartz substrate have been synthesized by seed-mediated growth approach in the presence of tannin.It was found that both the amount of tannin and the small triangular silver nanoplate seeds added to the growth solution are the key factors to modulation absorption band of triangular silver nanoplates.The optical in-plane dipole surface plasmon resonance (SPR) bands of these Ag nanoplates can be tuned from 608 nm to 980 nm via tannin deoxidization method.The formation mechanism of triangular silver nanoplates was proposed.The tannin deoxidization method realizes a convenient modulation of the absorption band of Ag nanostructures within the visible near-infrared (IR) region both in aqueous solvent and on substrates under mild conditions.
基金supported by the National Natural Science Foundation of China (21673088)~~
文摘Despite of extensive attention on the copper-based heterogeneous oxidative homocoupling of alkynes(OHA)to 1,3-diynes,the photocatalytic OHA is scarcely investigated.By screening copper-containing spinel catalysts,we discovered that a prereduced copper ferrite(CuFe2O4)not only can catalyze the thermocatalytic OHA but also is efficient for the photocatalytic OHA under visible light irradiation.It is found that the sol-gel combustion(SG)method and the partial reduction at 250 ℃ can result in the optimal CuFe2O4-SG-250 catalyst showing high activity and stability.Surface oxidized Cu2O is evidenced to be the active species for the thermocatalytic OHA,whereas metallic copper nanopaticles(CuNPs)are identified as the active sites for the photocatalytic OHA.The efficiency of photocatalytic OHA at ambient temperature is comparable to that of thermocatalytic OHA at 120 ℃,and the CuFe2O4-SG-250 catalyst can be magnetically separated and reused at least five times.The localized surface plasmon resonance effect of CuNPs contributes to visible light-induced photocatalytic OHA.
文摘Non-stoichiometric W_(18)O_(49)(WO)prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies.This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels.In addition,through the amination of CdSe,the one-dimensional/two-dimensional step-scheme(S-scheme)WO/CdSe-diethylenetriamine(WO/CdSe-D)photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method.The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency.The optimized photocatalyst of 35%WO/CdSe-D has the best CO_(2) reduction performance compared to WO and CdSe-D,and the yield is 25.37μmol h^(–1) g^(–1).X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction.This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO_(2) reduction.
文摘Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol(BA)into benzaldehydes(BAD)and H_(2),a novel localized surface plasmon resonance(LSPR)enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_(3-x) as oxidation semiconductor and Zn_(0.1)Cd_(0.9)S as reduction semiconductor.The photoredox system of Zn_(0.1)Cd_(0.9)S/MoO_(3-x) displayed an unconventional reaction model,in which the BA served as both electron donor and acceptor.The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically.Moreover,due to the LSPR effect of MoO_(3-x) nanosheets,Zn_(0.1)Cd_(0.9)S/MoO_(3-x) photocatalysts exhibited strong absorption in the region of full solar spectrum.Therefore,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite generated H_(2) and BAD simultaneously via selective oxidation of BA with high production(34.38 and 33.83 mmol×g^(–1) for H_(2) and BAD,respectively)upon full solar illumination.Even under NIR light irradiation,the H_(2) production rate could up to 94.5 mmol×g^(–1)×h^(–1).In addition,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite displayed effective photocatalytic H_(2) evolution rate up to 149.2 mmol×g^(–1)×h^(–1) from water,which was approximate 6 times that of pure Zn_(0.1)Cd_(0.9)S.This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
基金Supported by the Ministry of Science and Technology of China(No.2012YQ090194)the National Natural Science Foundation of China(No.51473115)
文摘A fast and facile method of fabricating fiber-optic localized surface plasmon resonance sensors baseff on spherical gold nanoparticles was introduced in this study. The gold nanoparticles with an average diameter of 55 nm were synthesized via the Turkevich method and were then immobilized onto the surface of an uncladded sensor probe using a polydopamine layer. To obtain a sensor probe with high sensitivity to changes in the refractive index, a set of key optimization parameters, including the sensing length, coating time of the potydopamine layer, and coating time of the gold nanoparticles, were investigated. The sensitivity of the optimized sensor probe was 522.80 nm per refractive index unit, and the probe showed distinctive wavelength shifts when the refractive index was changed from 1.328 6 to 1.398 7. When stored in deionized water at 4 ℃, the sensor probe proved to be stable over a period of two weeks. The sensor also exhibited advantages, such as low cost, fast fabrication, and simple optical setup, which indicated its potential application in remote sensing and real-time detection.
基金Supported by the National Natural Science Foundation of Tianjin (No. 09JCZDJC25700, 12JCZDJC29600 and KJXH2011-11)
文摘Lipoic acid (LA) has received great attention in the area of gold surface functionalization. In this study, LA was employed as a linker for the attachment of antibody to the gold surface of surface plasmon resonance (SPR) chip. By using this chip in a homemade SPR immunosensor, low molecular weight compound 2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD) can be detected at a low level of 0.01 ng/mL. There is a good linear relationship(R2 =0.943 1) between the results of SPR biosensor and enzyme-linked immunosorbent assay(ELISA).
基金Projects(20773165,20876179) supported by the National Natural Science Foundation of ChinaProject(09JJ1002) supported by the Hunan Provincial Natural Science Foundation,China+1 种基金Project(NCET-07-0865) for New Century Excellent Talents in Chinese UniversityProject(2007AA022006) supported by the National High Technology Research and Development Program of China
文摘To perform the mechanism study of special association for vancomycin and D-Ala-D-Ala-containing peptides on the interface of solution and self-assemble monolayer, the binding between vancomycin and pentapeptide （Lys-Lys-Gly-D-Ala-D-Ala） was investigated by flow injection surface plasmon resonance （FI-SPR） and flow injection quartz crystal microbalance （FI-QCM）. To facilitate the formation of a compact vancomycin adsorbates layer with a uniform surface orientation, vancomycin molecules were attached onto a preformed alkanethiol self-assembled monolayer. By optimizing the conditions for the binding between Lys-Lys-Gly-D-Ala-D-Ala and vancomycin on the assembled chip, the detecting limit of Lys-Lys-Gly-D-Ala-D-Ala was greatly improved （reaching 0.5 ×10^- 6 mol/L or 7.5 × 10^-12 mol）. The equilibrium constant of the association of Lys-Lys-Gly-D-Ala-D-Ala with vancomycin was also obtained （KAds=5.0×10^4 L/tool）.
基金supported by the National Natural Science Foundation of China under Grant Nos.10434060 and 10674047the Doctor Foundation of the Ministry of Education under Grant No.20040269010Shanghai Priority Academic Discipline,and the 211 Foundation of the Ministry of Education Doctor Program Scholarship Fund of ECNU 2007
文摘The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon resonance of small metallic particles. The role of energy transfer between ions and the particle is theoretical discussed. Depending on the particle size and the ion emission quantum efficiency, the enhancement of the absorption and the fluorescence is predicted. Moreover, taking Yb^3＋-doped ZBLAN as example, the cooling power and heat-light converting efficiency are calculated. It is finally concluded that the absorption and the fluorescence are greatly enhanced in these composite materials, the cooling power is increased compared to the bulk material.
文摘The n-type semiconducting titanium oxide thin films are well-known as electron transporting interlayer in photovoltaic cells. The favorable characteristics of interlayers in photovoltaics are high optical transmittance （T%）, wide band gap energy （Eg） and high electrical conductivity （σ）. Modifying titanium oxide films with metal nanoparticles would increase electrical conductivity but reduce optical band gap energy. We developed the sol-gel derived titanium suboxide （TiOx） films modified with silver （Ag） or gold （Au） or copper （Cu） nanoparticles （NPs）. This study explores a tradeoff between narrowing optical band gap and enhancing electrical conductivity of nanostructured TiOx films by controlling the Au- or Ag- or Cu-NPs loading concentrations （mol%） in titania. The Au- and Cu-NPs loading concentration of 4 mol% should meet a tradeoff which yields the higher T%, wider Eg and higher compared to those of pure TiOx films. In addition, since the pure Cu is not thermodynamically stable in ambience as compared to Au and Ag, the stability of as-obtained colloidal CuNPs is also examined. A careful examination of the time evolution of surface plasmon resonance （SPR） bands of CuNPs indicates that their stability is only up to 4 h.
基金Nature Science Foundation of Beijing,China(Grant No.7142088)
文摘Baicalein, baicalin, scutellarin and Chrysin-7-O-β-D-glucuronide are the major flavonoids of the Shuang-huang-lian powder injection. These flavonoids are thought to be haptens that can induce allergic reactions. The interaction mechanism of these haptens with bovine serum albumin （BSA） was investigated by surface plasmon resonance （SPR） and molecular modeling method. The SPR study indicated that these compounds could specifically bind to the BSA with one binding site and equilibrium dissociation constant （KD） values were determined. Molecular modeling explored the mechanism of interaction under simulated physiological condition. The result of molecular modeling indicated that flavonoids could bind with BSA in the hydrophobic pocket of sub-domain II with hydrogen bonding as the main acting force.
